WO2013110716A1 - Procédé et système de production de combustibles, d'une matière contenant du carbone à l'aide d'un gazéifieur de plasma - Google Patents

Procédé et système de production de combustibles, d'une matière contenant du carbone à l'aide d'un gazéifieur de plasma Download PDF

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WO2013110716A1
WO2013110716A1 PCT/EP2013/051360 EP2013051360W WO2013110716A1 WO 2013110716 A1 WO2013110716 A1 WO 2013110716A1 EP 2013051360 W EP2013051360 W EP 2013051360W WO 2013110716 A1 WO2013110716 A1 WO 2013110716A1
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gas
fuel
catalyst
reactor
carbon
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PCT/EP2013/051360
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English (en)
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Henrik SELSTAM
Erik Fareid
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Sge Scandgreen Energy Ab
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Priority to US14/373,926 priority Critical patent/US9199888B2/en
Publication of WO2013110716A1 publication Critical patent/WO2013110716A1/fr
Priority to US14/953,885 priority patent/US9856426B2/en

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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/02—Fixed-bed gasification of lump fuel
    • C10J3/06—Continuous processes
    • C10J3/18—Continuous processes using electricity
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
    • C01B3/12—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide
    • C01B3/16—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide using catalysts
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
    • C07C1/0405—Apparatus
    • C07C1/041—Reactors
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    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
    • C07C1/0485—Set-up of reactors or accessories; Multi-step processes
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/152—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the reactor used
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
    • C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
    • C10G2/34—Apparatus, reactors
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/002—Removal of contaminants
    • C10K1/003—Removal of contaminants of acid contaminants, e.g. acid gas removal
    • C10K1/004—Sulfur containing contaminants, e.g. hydrogen sulfide
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
    • C10K3/04—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment reducing the carbon monoxide content, e.g. water-gas shift [WGS]
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/02—Liquid carbonaceous fuels essentially based on components consisting of carbon, hydrogen, and oxygen only
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
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    • C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0255—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a non-catalytic partial oxidation step
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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    • C01B2203/06—Integration with other chemical processes
    • C01B2203/061—Methanol production
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    • C01B2203/06—Integration with other chemical processes
    • C01B2203/062—Hydrocarbon production, e.g. Fischer-Tropsch process
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1052—Nickel or cobalt catalysts
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    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1064—Platinum group metal catalysts
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    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1094—Promotors or activators
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
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    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0946—Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
    • C—CHEMISTRY; METALLURGY
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    • C10J2300/00—Details of gasification processes
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    • C10J2300/0953—Gasifying agents
    • C10J2300/0969—Carbon dioxide
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    • C10J2300/00—Details of gasification processes
    • C10J2300/12—Heating the gasifier
    • C10J2300/123—Heating the gasifier by electromagnetic waves, e.g. microwaves
    • C10J2300/1238—Heating the gasifier by electromagnetic waves, e.g. microwaves by plasma
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    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/1603—Integration of gasification processes with another plant or parts within the plant with gas treatment
    • C10J2300/1618—Modification of synthesis gas composition, e.g. to meet some criteria
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
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    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1659—Conversion of synthesis gas to chemicals to liquid hydrocarbons
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    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1662—Conversion of synthesis gas to chemicals to methane (SNG)
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    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1665—Conversion of synthesis gas to chemicals to alcohols, e.g. methanol or ethanol
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    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
    • C10L2290/04—Gasification
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
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    • C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
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    • C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
    • C10L2290/42—Fischer-Tropsch steps
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/10—Biofuels, e.g. bio-diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/141—Feedstock
    • Y02P20/145—Feedstock the feedstock being materials of biological origin
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/40—Ethylene production

Definitions

  • the present invention relates generally to the conversion of carbon containing waste materials into useful fuels. More specifically, the invention provides for methods, systems, and apparatus for the conversion of materials containing carbon to diesel and other useful fuels using synthesis gas as an intermediate.
  • synthesis gas Syngas
  • WO 2011/008263 A2 discloses the use of plasma gasification or pyrolysis for production of synthesis gas followed by the production of hydrogen from the synthesis gas in a water gas shift reaction and the production of products in various types of reactors.
  • WO 2011/002527 Al discloses a method in which syngas is generated from a waste and water using a plasma melter, hydrogen is extracted from the syngas using a water gas shift reaction, and a C9 fuel is synthesized from the extracted hydrogen and syngas in a Fischer- Tropsch type reactor.
  • the carbon for fuel synthesis is provided by the exhaust from a plant exhaust (e.g. a power plant exhaust), which is passed through a plasma chamber and then to a Fischer Tropsch reactor.
  • WO 2009/091325 Al discloses a biomass gasification method and apparatus for production of syngas with a rich hydrogen content; and US 5,584,255 discloses a method and apparatus for gasifying organic materials.
  • US 6,958,136 discloses a process for the treatment of nitrogen-containing waste streams that can generate syngas from carbon sources using alkalai metals and carbon radical formation.
  • Processes for synthesizing methane from syngas are known.
  • the methanation reaction converts syngas into methane and water in the presence of a catalyst (e.g. Ni/NiO, Ru, Cu, Pt, Rh) at temperatures between 150 °C and 600 °C.
  • a catalyst e.g. Ni/NiO, Ru, Cu, Pt, Rh
  • PCT/NO2007/000387 discloses a process for making methane from CO, C0 2 and H 2 involving the production of H 2 and 0 2 by splitting water.
  • Jianjun Guo et al. (2004) Applied Catalysis A: General 273(1-2): 75-82 discloses the production of methane over nickel catalyst on magnesium aluminate spines. M. Wisniewski et al.
  • Syngas may also be converted into a wide range of useful liquid hydrocarbons fuels and/or alcohols using the Fisher-Tropsch (F-T) process.
  • US 2007/0129449 discloses a method and installation for producing liquid energy carriers such as methanol from a solid carbon carrier. The method involves the production of 0 2 and H 2 by water electrolysis and gasifying a carbon carrier such as biomass or brown coal in a fluidized- bed gasifier in the presence of the produced 0 2 . The raw synthesis gas is transferred to a heat exchanger where the temperature is reduced and the cooled syngas is mixed with the produced H 2 to form methanol.
  • the production of hydrocarbon fuels such as diesel and gasoline are not described, however, and the installation as described is not suitable for F-T reactions forming diesel or gasoline.
  • WO 2008130260 Al discloses a waste to liquid hydrocarbon refinery system designed to convert municipal and industrial wastes, biomass, and other carbon-containing feedstocks into diesel, gasoline, and other products.
  • the system involves a high temperature liquid iron bed that generates raw syngas from solid and liquid feedstocks and a very high temperature plasmatron to convert contaminants in the raw syngas into ions.
  • a hydrocarbon synthesis subsystem converts the purified syngas into desired products.
  • the system is designed to minimize the release of toxic waste into the environment but is relatively complex and expensive, requires relatively large amount of energy, and releases considerable amounts of carbon into the atmosphere.
  • EP 0221679 A2 discloses a process for producing liquid hydrocarbons from biomass involving the production of synthesis gas from biomass and synthesizing liquid fuels from the produced synthesis gas.
  • Syngas is produced using a fluidized bed gasification system containing olefins.
  • Liquid fuel containing C7 to C17 paraffinic hydrocarbons is produced from the synthesis gas, along with propanol and water, using a catalytic liquefaction.
  • the process is designed to be economically viable but does not deal with pollutants such as NOx and SOx produced from biomass or the production of fuels from carbon-containing sources comprising municipal or industrial wastes.
  • the process is not designed to be carbon neutral.
  • the present invention in one or more aspects fills the aforementioned needs in the art by providing low emission and energy conserving systems and processes for producing useful fuels from a wide variety of carbon- containing source materials.
  • Embodiments of the present invention provide for a process, system and apparatus capable of using synthesis gas (CO + H 2 ) to produce methane, diesel fuel, and/or other hydrocarbons and useful energy.
  • a process according to the invention comprises the gasification and/or pyrolysis of a source material to produce synthesis gas using the produced synthesis gas for the production of a hydrocarbon, methanol, ammonia, urea, and other products using Fischer-Tropsch synthesis, methanation, and other reactions. Accordingly, embodiments of the present invention preferably seek to mitigate, alleviate or eliminate one or more deficiencies, disadvantages or issues in the art, singly or in any combination by providing carbon neutral methods and systems that produce
  • CO + H 2 synthesis gas
  • hydrocarbon fuels from carbon-containing materials especially carbon-containing waste materials such as bioorganic (biomass) waste and organic waste (e.g. plastics).
  • bioorganic waste materials such as bioorganic (biomass) waste and organic waste (e.g. plastics).
  • organic waste e.g. plastics.
  • a process and system for producing a hydrocarbon fuel comprises gasifying and/or pyrolizing a carbon source by plasma to form syngas; reacting a portion of the formed syngas with water in a water shift reactor to convert a portion of the syngas to C0 2 and H 2 and thereby adjust the ratio of CO to H 2 in the syngas; and synthesizing the hydrocarbon fuel from the produced syngas.
  • a process and system for producing a hydrocarbon fuel comprises gasifying and/or pyrolizing a carbon source by plasma to form C0 2 and H 2 0; reacting a portion of the formed C0 2 with H 2 to produce CO and H 2 and thereby adjust the ratio of CO to H 2 in the syngas; and synthesizing the hydrocarbon fuel from the produced CO and H 2 .
  • a process and a system for producing methanol comprises gasifying and/or pyrolizing a carbon source by plasma to form syngas; reacting a portion of the formed syngas with water to form C0 2 and H 2 to produce CO and H 2 ; and synthesizing methanol from the produced CO and H 2 .
  • a process and system for producing a hydrocarbon fuel comprises gasifying and/or pyrolizing a carbon source by plasma to form CO and H 2 , and synthesizing the hydrocarbon fuel from the produced CO and H 2 .
  • a process and system for producing a ammonia comprises gasifying and/or pyrolizing a carbon source by plasma to form CO and H 2 ; reacting all or a portion of the formed CO with water to produce H 2; and synthesizing ammonia from the produced H 2 and nitrogen.
  • Additional aspects of the invention include methods, apparatus, and systems comprising combinations of the aspects of the invention to produce methane, methanol, diesel, and other chemicals; to perform Fischer-Tropsch processes, provide gas turbine fuel, and for carbon capture and storage (CCS).
  • CCS carbon capture and storage
  • Gasification/pyrolysis may be performed by any suitable means, preferably a plasma gasification means, including cool plasma and plasma gasification.
  • Thermal catalytic gasification methods such as counter-current fixed bed (“up draft”) gasification, co- current fixed bed (“down draft”) gasification, fluidized bed gasification and entrained flow gasification are not suitable gasification means because synthesis gas produced using these gasification means may contain large amounts of tar that fowl catalytic systems.
  • Heat from reactions of synthesis gas may supply all or parts of the heat required to gasify or pyrolize carbon-containing source materials such as biological and organic waste to form synthesis gas. Through this process it is possible to gasify organic and biological waste and produce energy in a C0 2 neutral manner.
  • a "reaction loop" is formed, wherein the recapture of heat produced by chemical reactions provides usable energy as electrical energy or chemical energy in the form of a fluid that may be combusted directly or stored as potential chemical energy.
  • An advantage of the present system and process is the reduction of C0 2 emissions with respect to existing gas to fuel systems and the possibility of achieving carbon neutral carbon source to fuel conversion.
  • Another advantage of the present invention is the ability to reduce mixed oxides of nitrogen and sulfur (NOx and SOx) to nitrogen, water, and sulfur and thereby reduce or eliminate emissions of these pollutants.
  • Yet another advantage of the present invention is the selective synthesis of hydrocarbon species in a gas to fuel reaction, such as the selective synthesis of Cg-C 14 hydrocarbons, by controlling catalyst composition and reactions conditions.
  • Yet another advantage of the present invention is the ability to use raw synthesis gas produced by plasma gasification directly for water shift and/or gas to fuel reactions to produce liquid fuel.
  • neutral with respect to emitted C0 2 means that total carbon emission to the atmosphere neither increases nor reduces during a process.
  • a carbon neutral process is plants assimilating carbon (in the form of C0 2 ) from the atmosphere and storing it in the form of cellulose, sugars, or other biomass and the combustion of the biomass in air to produce the same amount of C0 2 as was assimilated by the plants.
  • organic waste refers to all waste containing organic chemicals containing carbon and hydrogen. Examples of organic waste include municipal solid waste, plastics, sewage, animal manure, and hospital waste.
  • biological waste refers to any waste of biological origin containing carbon and hydrogen.
  • biological waste include olive pits, rice husks, bagasse, wood chips, sawdust, corn husks, and products and byproducts of agricultural and/or forestry processes including methane gas.
  • hydrocarbon fuels refers to materials comprising any number of carbon atoms and hydrogen atoms that may react through combustion to producing energy.
  • hydrocarbon fuels include methane, methanol, ethanol, propane, butane, diesel, gasoline, and kerosene.
  • Hydrocarbon fuels include alkanes, alcohols, alkenes, alkynes, and aromatic
  • carbon-containing source material refers to materials comprising any number carbon atoms and hydrogen atoms in their structure that may be converted to or processed to a fluid or gaseous form or which may remain in a solid form, and which in their solid, fluid or gaseous forms may be combusted to form carbon monoxide and/or carbon dioxide and/or methane.
  • Non-limiting examples of carbon-containing source materials include organic and biological waste as described supra, and any waste containing carbon that may be used as material for a pyrolysis or gasification process including but not limited to solid or liquid municipal waste, solid or liquid biomass, solid or liquid medical waste, solid or liquid biohazard waste, solid or liquid chemical waste, and coal.
  • combustion refers to any reaction involving oxygen and a carbonaceous material within the temperature intervals indicated infra.
  • gasification means the evaporation and/or combustion of organic fuel by cool plasma gasification or plasma gasification.
  • chemical energy refers to the latent or potential energy of a compound that may be released through a chemical process that lowers the potential energy of the relevant compound forming one or more reaction products with a lower net potential energy and releasing the energy difference between the original compound(s) and the product(s).
  • electrical energy refers to energy that may be utilized by an electrical storage unit (battery, condenser, etc.) or be converted to other forms of energy, e.g. mechanical energy, through the use of an electrical appliance.
  • the term “large amounts of energy” refers to energy within the range 5-50 MJ/kg.
  • the term “large amounts” of chemical energy in the context of the present invention is an energy difference between original and product compounds that represents at least 15% of the chemical energy of the original compound(s).
  • the term "about” refers to a relative deviation from the indicated amount of up to + 10%, i.e. an interval of one unit per ten units of the relevant number.
  • the deviation may also be smaller, e.g. 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8% or 9% or any number in between or any interval combination thereof.
  • Fig. 1 is schematic of a system and process for gasification of biomass using air as a gasification gas
  • Fig. 2 is schematic of a Gas to Fuel Process system and process for the production of diesel.
  • the invention is not limited to this application but may be applied to the synthesis of many other products including, for example jet fuel, gasoline, propane, butane, ammonia, urea, ethanol, and propanol.
  • a first stage in one embodiment according to the invention comprises the production of synthesis gas from a carbon-containing material by gasification and/or pyrolysis.
  • a process and system for the first stage of such an embodiment is shown in FIG. 1.
  • This embodiment of the invention provides for energy recapture to provide usable energy as well as providing a gas that may be combusted or that contains large amounts of chemical energy.
  • a feed of carbon-containing source material 101 is mixed with a feed of air, steam, and/or an oxygen-containing gas 102 in a mixer 103 and introduced into a gasifier 104.
  • the gasifier 104 is configured to produce a feed comprising CO and H 2 (syngas) 105.
  • gasifiers that are suitable for commercial production of clean syngas according to the invention include cool plasma gasifiers and plasma gasifiers.
  • the first stage of the process shown in FIG. 1 may comprise catalysts and other devices that produce syngas. Syngas contains H 2 and CO and, depending on the source materials and reactions, may also contain on or more of C0 2 , H 2 0, N 2 , NOx, SOx, and CH 4 .
  • Cool plasma gasification or pulsed plasma gasification effectively breaks down organic molecules into synthesis gas. Unlike gasifiers that rely solely on heat to provide molecular disassociation, temperature plays only a partial role in cool-plasma gasification.
  • a plasma field is created in an oxygen-starved environment that generates a temperature of approximately 1,300°C at the bottom end of the plasma arc spectrum. Biomass or organic waste is passed directly through the plasma field in such a way that both temperature and plasma dynamics combine to accomplish molecular disassociation.
  • the plasma field is pulsed to create shock waves and molecular temperatures as high as 15,000 °C to 50,000 °C, while the average temperature is maintained at 1300°C.
  • the shock waves and high temperatures break down longer and complex molecular chains, resulting in the reduction of the raw feedstock into its elemental components.
  • the relatively low average temperature allows an energy recovery of around 90%.
  • Plasma gasification is used to break down waste materials that are infectious or in other ways pose an environmental hazard.
  • High voltage, high current electricity is passed between two electrodes that are spaced apart, creating an electrical arc. Consequently, the process is more expensive and is associated with lower energy recovery (around 50%) than cool plasma gasification.
  • Inert gas or gas with low oxygen content under pressure is passed through the arc into a sealed container of waste material.
  • the temperature may be as high as 14,000°C in the arc column, while the temperature a few feet from the torch can be as high as 2800 °C -5000 °C. At these temperatures, most wastes are dissociated into elemental components in a gaseous form.
  • the reactor operates at a slightly negative pressure, meaning that the feed system is complemented by a gas removal system, and also a solid removal system.
  • gas from the plasma containment can be removed as syngas, and may be refined into various fuels at a later stage or used on site to provide power.
  • Syngas is produced from organic materials with a conversion rate of greater than 99% using plasma gasification. Inorganic materials in the waste stream that are not broken down undergo a phase change (e.g. from solid to liquid) to form a slag. A portion of the syngas may be used to run an on-site turbine to power plasma torches and feed systems.
  • Gasification of organic material according to the present invention is preferably performed with low levels of 0 2 , i.e. 0 2 concentrations of the inlet gas in the range of 0.5%- 15% 0 2 (v/v), but may also be performed by using exhaust gas, from a
  • Gasification of the carbon-containing source material may be performed at a temperature in the range of 500 °C-5000 °C, preferably within the range of 1000-5000°C, e.g. within the range of 500°C-1000°C, 1000° -1500°C, 1500°C-2500°C, 2500°C-3500°C, or 3500°C -5000°C.
  • the gasification pressure may range from 0.5 bar to 10 bar.
  • the temperature of the syngas feed leaving the gasifier may be in the range of 100 °C - 2000 °C, depending on the conditions and starting materials selected. Examples of selected temperature ranges for the combustion products include 200 °C -1800 °C, 300 °C -1500 °C, 400 °C -1300 °C, 500 °C -1250 °C, 550 °C -1200 °C, 600 °C -1100 °C, 700 °C - 1000°C or any combination of these. If the temperature of the synthesis gas leaving the gasifier is high enough, a heat exchanger 106 may be used to generate electrical energy or supply heat for producing steam and to produce a cooled syngas feed 107. Water that may be present in cooled syngas feed 107 may be removed in separator 108 to separate condensed water 109 from syngas feed 110.
  • Syngas feed 110 is mixed with steam 113 in mixer 112 to form a mixture of steam, H 2 , and CO 114, which enters a water gas shift reactor 115 where the steam and CO react to form C0 2 and H 2 .
  • the operation of the water gas shift reactor 115 may be controlled to produce a syngas feed having a desired H 2 :CO ratio which may range, for example, from 1:4 to 4: 1.
  • the final ratio may be selected based upon the fuel to be synthesized in the second stage of the process.
  • the shift reaction may occur in a low temperature reactor or a high temperature reactor wherein CO reacts with steam over a suitable catalyst to produce C0 2 and H 2 .
  • suitable catalysts are iron oxide/chromium oxide and copper oxide/zinc oxide catalysts for low and high temperature reactors, respectively.
  • the produced syngas which now comprises H 2 and CO in a desired ratio, e.g. 2: 1, and C0 2 , provides a syngas feed 116 for a second stage of the process shown in FIG. 2.
  • a heat exchanger 106 may be placed downstream of water gas shift reactor 115 to be used as the heat exchanger upstream of separator 108 and may also be used to maintain products of the reactor 115 at a desired temperature.
  • a gasification system that produces a synthesis gas comprising H 2> CO, and C0 2 having a desired H 2 :CO ratio by proper selection of, for example, the carbon-containing material for gasification, the concentration of oxygen present during gasification, the amount of water present in the carbon-containing material and/or during gasification, to effectively combine the water gas shift reaction into the gasification process.
  • the water gas shift reactor may be dispensed with and the synthesis gas produced by gasification may be used to provide a synthesis gas feed stream 116 for a second stage of the process shown in FIG. 2.
  • FIG. 2 A system for performing a second stage of a process according to the invention is shown in FIG. 2.
  • a syngas feed 116 is compressed by a compressor 117 before being conveyed into a gas to fuel reactor 118 where the syngas is converted to a fuel- containing feed stream 119.
  • the embodiment shown comprises a two stage compressor 117 comprising two compressors 117a, 117b with an optional heat exchanger 117c located between the two compressors to remove heat and cool the syngas to a temperature of.
  • the compressor however, need not be a two-stage compressor, which is used for the purpose of describing this specific embodiment of the invention.
  • the gas to fuel reactor 118 is shown comprising two rector vessels 118a and 118b but other embodiments may comprise more of fewer reactors (reactor vessels) arranged in series and/or in parallel and performing the same of different chemical reactions.
  • an optional heat exchanger 120 which may be integrated in the reactor 118, may be used to cool the fuel-containing feed stream 119 and provide heat for electrical energy production and plasma gasifier operation and/or heat for steam production.
  • the embodiment shown in FIG. 2 may be configured, for example, for the production of gasoline, kerosene, and/or diesel by exothermic reactions. While embodiments for the production of diesel and other specified fuels are described herein, the invention is not intended to be limited to the specific embodiments described.
  • the cooled fuel-containing feed 119 may contain, in addition to diesel, methane, ethane, C0 2 , and unreacted syngas.
  • the cooled fuel-containing feed stream 119 is conveyed to and expanded in turbine 121, optionally cooled in heat exchanger 122, and separated into liquid and gaseous components 124, 128 in separator 123.
  • the gaseous components 128, including methane, ethane, C0 2 , and syngas are mixed with an air feed 102 in mixer 129 and conveyed to a power generator 130 where they are combusted to provide, for example, electrical energy and combustion products 131.
  • the liquid components 124 may be conveyed to a distillation apparatus 125 where diesel, water, and other liquid components are separated to produce diesel and water outlet streams 126, 127.
  • the diesel synthesis reaction performed in the gas to fuel reactor 118 preferably uses a gas composition comprising a H 2 /CO ratio of about 2.
  • the primary reaction for the formation of diesel from synthesis gas is:
  • n has a value of 14 - 20.
  • other products may be formed, such as higher alcohols and hydrocarbons.
  • the selectivity of known catalysts for the reaction is over 80%.
  • Diesel synthesis is performed at pressures above 25 bar at temperatures normally not exceeding 570K.
  • the ratio of H 2 may be controlled by the water gas shift reactor 115. Additionally or alternatively, the ratio of H 2 /CO may be adjusted by providing an additional hydrogen-rich feed from a source of hydrogen production.
  • the catalyst in the gas to fuel reactor 118 comprises Fe metal alloyed with Co metal and/or Ru metal coated on a support and comprising an amount of a promoter selected from the group of Pd, Pt, Cu, Rh, Ir, Ag, W, Ir, and combinations thereof.
  • the weight percent of Fe, Co, and or Ru present in the catalyst is 20-80%.
  • the weight percent of promoter in the catalyst may range from 0.01%-10% or preferably 0.01% to 1.0%.
  • the same catalyst may be, but need not be, used in both the water gas shift reactor 115 and the gas to fuel reactor 118. It is also possible to perform the water gas shift reaction and the gas to fuel reaction simultaneously in a single reactor.
  • synthesis gas may be converted to a wide range of hydrocarbons and/or alcohols in gas to fuel reactor 118 through one or more F-T process reactions:
  • Alcohols* nCO + 2nH 2 ⁇ H(-CH 2 -) n OH + (n- 1 )H 2 0
  • F-T reactions are highly exothermic. For example, the formation of 1 mol of -CH 2 - is accompanied by a release of 165 kJ/mol of heat.
  • the reaction performed in reactor 118 may also be a methanation reaction performed in the presence of Ni/NiO, Ru, Cu, Pt, Rh, Ag, Co, and/or W catalyst in the temperature range of 150 °C to 600 °C and pressures of from 1 bar to 50 bar.
  • CO and C0 2 react with H 2 to form methane and water according to Methanation Reactions 2 and 3 in Table 1.
  • the catalyst may also suppress the reverse shift reaction 4.
  • the methane produced may be used as a fuel or as a raw material for the production of methane, diesel, ammonia, urea, nitric acid, ammonium nitrate, NPK, and PVC, for example.
  • Reactors for these syntheses may be coupled to a fuel outlet 126 (FIG. 2) in an embodiment producing methane.
  • the H 2 and CO produced may also be used as raw materials for other uses and processes.
  • the processes according to the present invention may be performed within a reactor for providing ways of controlling the physical and chemical parameters involved in the reaction equations shown in Table 1.
  • a reactor producing H 2 and CO according to reaction 5 may provide H 2 to a reaction vessel that is provided with additional H 2 , directly or indirectly, from a reaction vessel producing H 2 in which reaction 1 takes place.
  • Produced H 2 may also be reacted with CO and C0 2 in a single or in separate reaction vessels according to reaction 2 and 3 to produce methane.
  • the reactions and reaction vessels in the gas to fuel reactor may be configured according to the product(s) to be synthesized using reactions 1-7 in Table 1 without relying on energy consuming processes for producing H 2 such as water splitting.
  • the system and process may comprise more than one gasifier 104, for example arranged in parallel, using different carbon source materials and or different oxygen
  • the different streams of syngas may be blended in a controlled manner before being fed into, for example, gas to fuel reactor(s) 118.
  • Reacting CO and/or C0 2 with H 2 to produce methane may be performed in a single reactor with a catalyst.
  • the heat developed may be used for gasification, steam production, and/or generating electricity.
  • the shape of the catalyst is not critical and may inter alia comprise coated monoliths, nano materials, and/or other types and forms of carriers.
  • the carriers may be selected from e.g. Ti0 2 , A1 2 0 3 , cordierite, and Gd- doped CeO.
  • the catalytic material may also be present in any form as a "pure" catalyst material.
  • the form and composition of the reactor and the catalyst depends on the source of CO and/or C0 2 . If the source is an impure exhaust gas with large amounts of dust (e.g.
  • a monolithic catalyst carrier may be used, whereas a catalyst in the form of pellets may be used with a pure exhaust gas (e.g. from a natural gas turbine). All types of exhaust gases from all types of combustions of organic material may be used as a source material for the second stage gas to fuel reactor 118 (FIG. 2) to produce methane.
  • a monolithic catalyst carrier may be used, whereas a catalyst in the form of pellets may be used with a pure exhaust gas (e.g. from a natural gas turbine). All types of exhaust gases from all types of combustions of organic material may be used as a source material for the second stage gas to fuel reactor 118 (FIG. 2) to produce methane.
  • a catalyst in the form of pellets may be used with a pure exhaust gas (e.g. from a natural gas turbine). All types of exhaust gases from all types of combustions of organic material may be used as a source material for the second stage gas to fuel reactor 118 (FIG. 2) to produce methane.
  • nitrogen containing compounds such as ammonia and urea using known chemical syntheses.
  • H 2 may be separated from CO and/or C0 2 produced by gasifier 104 and reacted with oxygen depleted air or nitrogen in an exhaust gas:
  • the present invention is also useful for the sequestration of C0 2 produced by the burning of fossil fuels.
  • C0 2 may react with carbon in the carbon-containing source material to form CO, which is ultimately used in the gas to fuel reactor 118 to produce diesel fuel, for example.
  • C0 2 produced by fossil fuel combustion may alternatively or additionally enter the process/system in stream 102 (FIG. 1) with or without addition of air and/or oxygen and/or steam.
  • a fossil fuel is combusted with air in a burner or combustor and electricity is produced from the combustion process in a conventional manner.
  • the exhaust, containing H 2 0 and C0 2 is cooled to condense and remove H 2 0.
  • C0 2 in the combustion gas is about 1-20 % by volume.
  • C0 2 from the exhaust is used as a feed in addition to feed 116 into reactor 118 for methane production according to reaction 3 or reactions 2 and 3 in Table 1.
  • the methane produced is recirculated while the hydrogen and CO produced by the gasification is used for producing methanol.
  • NOx nitrogen-containing gases
  • SOx may also be present in a gasification or pyrolysis exhaust gas.
  • An advantage of the present process is that these pollutants can be reduced to elemental nitrogen and sulfur in the gas to fuel reactor(s) 118 and thereby reduce air pollution compared to existing processes. Reduction of NOx and SOx may be achieved by one or more of the following reactions with synthesis gas:
  • Sulfur present in an exhaust stream from the combustion of high sulfur coal, sulfur containing biomass, or sulfur containing municipal waste may be reduced by reaction with carbon in a gasifier 104 or additional gasifier according to the reaction

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Abstract

La présente invention concerne un procédé et un système de production de combustibles liquides et gazeux et d'autres produits chimiques utiles à partir de carbone contenant des matériaux source qui consiste en la gazéification de plasma froid et/ou la pyrolyse d'un matériau source pour produire un gaz de synthèse à l'aide du gaz de synthèse produit pour la production d'un hydrocarbure, de méthanol, d'ammoniac, d'urée, et d'autres produits. Le procédé et le système sont capables de séquestrer du dioxyde de carbone et de réduire du NOx et du SOx.
PCT/EP2013/051360 2012-01-24 2013-01-24 Procédé et système de production de combustibles, d'une matière contenant du carbone à l'aide d'un gazéifieur de plasma WO2013110716A1 (fr)

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